Ye, C.Shan, J.Chao, D.Liang, P.Jiao, Y.Hao, J.Gu, Q.Davey, K.Wang, H.Qiao, S.2021-11-042021-11-042021Journal of the American Chemical Society, 2021; 143(41):16902-169070002-78631520-5126https://hdl.handle.net/2440/132923Potassium–sulfur batteries hold practical promise for next-generation batteries because of their high theoretical gravimetric energy density and low cost. However, significant impediments are the sluggish K2S oxidation kinetics and a lack of atomic-level understanding of K2S oxidation. Here, for the first time, we report the catalytic oxidation of K2S on a sulfur host with Co single atoms immobilized on nitrogen-doped carbon. On the basis of combined spectroscopic characterizations, electrochemical evaluation, and theoretical computations, we show a synergistic effect of dynamic Co–S and N–K interactions to catalyze K2S oxidation. The resultant potassium–sulfur battery exhibited high capacities of 773 and 535 mAh g–1 under high current densities of 1 and 2 C, respectively. These findings provide atomic-scale insights for the rational design of highly efficient sulfur hosts.en© 2021 American Chemical SocietyJournal article10.1021/jacs.1c062552021-11-04589815Shan, J. [0000-0003-4308-5027]Chao, D. [0000-0001-7793-0044]Jiao, Y. [0000-0003-1329-4290]Hao, J. [0000-0002-5777-7844]Davey, K. [0000-0002-7623-9320]Qiao, S. [0000-0002-1220-1761] [0000-0002-4568-8422]